H. De Backer

In-situ measurements of stratospheric ozone depletion rates in the Arctic winter 1991/1992: A Lagrangian approach

A Lagrangian approach has been used to assess the degree of chemically induced ozone loss in the Arctic lower stratosphere in winter 1991/1992. Trajectory calculations are used to identify air parcels probed by two ozonesondes at different points along the trajectories. A statistical analysis of the measured differences in ozone mixing ratio and the time the air parcel spent in sunlight between the measurements provides the chemical ozone loss. Initial results were first described by von der Gathen et al. [1995]. Here we present a more detailed description of the technique and a more comprehensive discussion of the results. Ozone loss rates of up to 10 ppbv per sunlit hour (or 54 ppbv per day) were found inside the polar vortex on the 475 K potential temperature surface (about 19.5 km in altitude) at the end of January. The period of rapid ozone loss coincides and slightly lags a period when temperatures were cold enough for type I polar stratospheric clouds to form. It is shown that the ozone loss occurs exclusively during the sunlit portions of the trajectories. The time evolution and vertical distribution of the ozone loss rates are discussed.

Changes in ozone over Europe: Analysis of ozone measurements from sondes, regular aircraft (MOZAIC) and alpine surface sites

We use ozone observations from sondes, regular aircraft, and alpine surface sites in a self-consistent analysis to determine robust changes in the time evolution of ozone over Europe. The data are most coherent since 1998, with similar interannual variability and trends. Ozone has decreased slowly since 1998, with an annual mean trend of −0.15 ppb yr−1 at ∼3 km and the largest decrease in summer. There are some substantial differences between the sondes and other data, particularly in the early 1990s. The alpine and aircraft data show that ozone increased from late 1994 until 1998, but the sonde data do not. Time series of differences in ozone between pairs of locations reveal inconsistencies in various data sets. Differences as small as few ppb for 2-3 years lead to different trends for 1995-2008, when all data sets overlap. Sonde data from Hohenpeissenberg and in situ data from nearby Zugspitze show ozone increased by ∼1 ppb yr−1 during 1978-1989. We construct a mean alpine time series using data for Jungfraujoch, Zugspitze, and Sonnblick. Using Zugspitze data for 1978-1989, and the mean time series since 1990, we find that the ozone increased by 6.5-10 ppb in 1978-1989 and 2.5-4.5 ppb in the 1990s and decreased by 4 ppb in the 2000s in summer with no significant changes in other seasons. It is hard to reconcile all these changes with trends in emissions of ozone precursors, and in ozone in the lowermost stratosphere. We recommend data sets that are suitable for evaluation of model hindcasts.

Chemical depletion of Arctic ozone in winter 1999/2000

During Arctic winters with a cold, stable stratospheric circulation, reactions on the surface of polar stratospheric clouds (PSCs) lead to elevated abundances of chlorine monoxide (ClO) that, in the presence of sunlight, destroy ozone. Here we show that PSCs were more widespread during the 1999/2000 Arctic winter than for any other Arctic winter in the past two decades. We have used three fundamentally different approaches to derive the degree of chemical ozone loss from ozonesonde, balloon, aircraft, and satellite instruments. We show that the ozone losses derived from these different instruments and approaches agree very well, resulting in a high level of confidence in the results. Chemical processes led to a 70% reduction of ozone for a region ∼1 km thick of the lower stratosphere, the largest degree of local loss ever reported for the Arctic. The Match analysis of ozonesonde data shows that the accumulated chemical loss of ozone inside the Arctic vortex totaled 117 ± 14 Dobson units (DU) by the end of winter. This loss, combined with dynamical redistribution of air parcels, resulted in a 88 ± 13 DU reduction in total column ozone compared to the amount that would have been present in the absence of any chemical loss. The chemical loss of ozone throughout the winter was nearly balanced by dynamical resupply of ozone to the vortex, resulting in a relatively constant value of total ozone of 340 ± 50 DU between early January and late March. This observation of nearly constant total ozone in the Arctic vortex is in contrast to the increase of total column ozone between January and March that is observed during most years.

Validation of Aura Microwave Limb Sounder Ozone by ozonesonde and lidar measurements

We present validation studies of MLS version 2.2 upper tropospheric and stratospheric ozone profiles using ozonesonde and lidar data as well as climatological data. Ozone measurements from over 60 ozonesonde stations worldwide and three lidar stations are compared with coincident MLS data. The MLS ozone stratospheric data between 150 and 3 hPa agree well with ozonesonde measurements, within 8% for the global average. MLS values at 215 hPa are biased high compared to ozonesondes by A`20% at middle to high latitude, although there is a lot of variability in this altitude region. Comparisons between MLS and ground-based lidar measurements from Mauna Loa, Hawaii, from the Table Mountain Facility, California, and from the Observatoire de Haute-Provence, France, give very good agreement, within A`5%, for the stratospheric values. The comparisons between MLS and the Table Mountain Facility tropospheric ozone lidar show that MLS data are biased high by A`30% at 215 hPa, consistent with that indicated by the ozonesonde data. We obtain better global average agreement between MLS and ozonesonde partial column values down to 215 hPa, although the average MLS values at low to middle latitudes are higher than the ozonesonde values by up to a few percent. MLS v2.2 ozone data agree better than the MLS v1.5 data with ozonesonde and lidar measurements. MLS tropical data show the wave one longitudinal pattern in the upper troposphere, with similarities to the average distribution from ozonesondes. High upper tropospheric ozone values are also observed by MLS in the tropical Pacific from June to November.

Chemical Ozone Loss in the Arctic Winter 1994/95 as Determined by the Match Technique

The chemically induced ozone loss inside the Arctic vortex during the winter 1994/95 has been quantified by coordinated launches of over 1000 ozonesondes from 35 stations within the Match 94/95 campaign. Trajectory calculations, which allow diabatic heating or cooling, were used to trigger the balloon launches so that the ozone concentrations in a large number of air parcels are each measured twice a few days apart. The difference in ozone concentration is calculated for each pair and is interpreted as a change caused by chemistry. The data analysis has been carried out for January to March between 370 K and 600 K potential temperature. Ozone loss along these trajectories occurred exclusively during sunlit periods, and the periods of ozone loss coincided with, but slightly lagged, periods where stratospheric temperatures were low enough for polar stratospheric clouds to exist. Two clearly separated periods of ozone loss show up. Ozone loss rates first peaked in late January with a maximum value of 53 ppbv per day (1.6 % per day) at 475 K and faster losses higher up. Then, in mid-March ozone loss rates at 475 K reached 34 ppbv per day (1.3 % per day), faster losses were observed lower down and no ozone loss was found above 480 K during that period. The ozone loss in hypothetical air parcels with average diabetic descent rates has been integrated to give an accumulated loss through the winter. The most severe depletion of 2.0 ppmv (60 %) took place in air that was at 515 K on 1 January and at 450 K on 20 March. Vertical integration over the levels from 370 K to 600 K gives a column loss rate, which reached a maximum value of 2.7 Dobson Units per day in mid-March. The accumulated column loss between 1 January and 31 March was found to be 127 DU (∼36 %).

A trajectory-based estimate of the tropospheric ozone column using the residual method

We estimate the tropospheric column ozone using a forward trajectory model to increase the horizontal resolution of the Aura Microwave Limb Sounder (MLS) derived stratospheric column ozone. Subtracting the MLS stratospheric column from Ozone Monitoring Instrument total column measurements gives the trajectory enhanced tropospheric ozone residual (TTOR). Because of different tropopause definitions, we validate the basic residual technique by computing the 200-hPa-to-surface column and comparing it to the same product from ozonesondes and Tropospheric Emission Spectrometer measurements. Comparisons show good agreement in the tropics and reasonable agreement at middle latitudes, but there is a persistent low bias in the TTOR that may be due to a slight high bias in MLS stratospheric column. With the improved stratospheric column resolution, we note a strong correlation of extratropical tropospheric ozone column anomalies with probable troposphere-stratosphere exchange events or folds. The folds can be identified by their colocation with strong horizontal tropopause gradients. TTOR anomalies due to folds may be mistaken for pollution events since folds often occur in the Atlantic and Pacific pollution corridors. We also compare the 200-hPa-to-surface column with Global Modeling Initiative chemical model estimates of the same quantity. While the tropical comparisons are good, we note that chemical model variations in 200-hPa-to-surface column at middle latitudes are much smaller than seen in the TTOR.

Distribution of ozone laminae during EASOE and the possible influence of inertia-gravity waves

The distribution of laminae in ozone has been determined from the EASOE ozonesonde archive as a function of potential temperature and potential vorticity. Results confirm previous studies that laminae are absent above ∼450K within the vortex, and are most abundant near its edge. Observations of inertia-gravity waves in the lower stratosphere appear to suggest that such waves are not of sufficiently large amplitude to cause the kinds of laminae that are observed.

Arctic Ozone Loss in Threshold Conditions: Match Observations in 1997/1998 and 1998/1999

Chemical ozone loss rates inside the Arctic polar vortex were determined in early 1998 and early 1999 by using the Match technique based on coordinated ozonesonde measurements. These two winters provide the only opportunities in recent years to investigate chemical ozone loss in a warm Arctic vortex under threshold conditions, i.e., where the preconditions for chlorine activation, and hence ozone destruction, only occurred occasionally. In 1998, results were obtained in January and February between 410 and 520 K. The overall ozone loss was observed to be largely insignificant, with the exception of late February, when those air parcels exposed to temperatures below 195 K were affected by chemical ozone loss. In 1999, results are confined to the 475 K isentropic level, where no significant ozone loss was observed. Average temperatures were some 8°–10° higher than those in 1995, 1996, and 1997, when substantial chemical ozone loss occurred. The results underline the strong dependence of the chemical ozone loss on the stratospheric temperatures. This study shows that enhanced chlorine alone does not provide a sufficient condition for ozone loss. The evolution of stratospheric temperatures over the next decade will be the determining factor for the amount of wintertime chemical ozone loss in the Arctic stratosphere.

Match observations in the Arctic winter 1996/97: High stratospheric ozone loss rates correlate with low temperatures deep inside the polar vortex

With the Match technique, which is based on the coordinated release of ozonesondes, chemical ozone loss rates in the Arctic stratospheric vortex in early 1997 have been quantified in a vertical region between 400 K and 550 K. Ozone destruction was observed from mid February to mid March in most of these levels, with maximum loss rates between 25 and 45 ppbv/day. The vortex averaged loss rates and the accumulated vertically integrated ozone loss have been smaller than in the previous two winters, indicating that the record low ozone columns observed in spring 1997 were partly caused by dynamical effects. The observed ozone loss is inhomogeneous through the vortex with the highest loss rates located in the vortex centre, coinciding with the lowest temperatures. Here the loss rates per sunlit hour reached 6 ppbv/h, while the corresponding vortex averaged rates did not exceed 3.9 ppbv/h.

Revision of 20 years of Dobson total ozone data at Uccle (Belgium): Fictitious Dobson total ozone trends induced by sulfur dioxide trends

Since July 1971, total ozone measurements have been performed at Uccle (50°48′N, 4°21′E) with the Dobson spectrophotometer 40. All the individual measurements were reevaluated after a careful homogenization, using the detailed calibration history of the instrument. Special care was taken to assure the consistency between direct Sun (DS) and zenith sky (ZS) measurements. The monthly mean values of percentage differences between the quasi-simultaneous direct Sun and zenith sky measurements show a weak modulation, probably induced by long-term changes in the mean vertical ozone distribution. The overall standard deviation of the percentage differences between the two types of observations amounts to 1.72%. From a detailed comparison of our revised data over the period 1971–1986 with the results of an approximate revision on a month-by-month basis (used in the Report of the International Ozone Trends Panel), it is concluded that the latter method of revision is not reliable. The trend of the reduced thickness of the SO2 amount in the lower troposphere, as measured with the Brewer instrument 16 located at the same site as the Dobson spectrophotometer, is in agreement with the trend of the SO2 density near the ground which has been measured in the urban area of Brussels since 1968. From these two SO2 data sets the variation of the reduced SO2 amount since 1968 and the corresponding correction of the Dobson instrument data of Uccle were calculated on a month-by-month basis. Without the SO2 correction the revised Dobson data for the period from August 1971 through July 1991 show a statistically significant downward trend (± standard deviation) that amounts to −1.38 ± 0.50% per decade, while after the SO2 correction a nonsignificant trend of 0.31 ± 0.51% per decade is found. This means that the decrease of SO2 over the last two decades at Uccle has induced a fictitious Dobson total ozone trend of −1.69% per decade. At the subperiod for which reprocessed total ozone mapping spectrometer (TOMS) data are available (November 1978 to May 1990) our corrected Dobson data show a statistically significant downward trend (± standard deviation) of −2.93 ± 1.17% per decade which is consistent with the results from TOMS; this proves that analysis of total ozone data over time periods as short as one solar cycle does not allow to make conclusive statements about long-term trends. The spectacular decrease of SO2 densities is not a regional phenomenon but has been generally ascertained in European and North American urban areas; therefore it should not be neglected in any study about global ozone trends derived from Dobson data.